Min Chul Choi, Wooil Yang, Young-Woo Son, Se Young Park
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引用次数: 0
摘要
我们使用从头算扩展Hubbard泛函(DFT + U + V)研究了铁电钙钛矿氧化物BaTiO3、PbTiO3、LiNbO3和BiFeO3的原子和电子结构,其中现场和现场间的Hubbard参数是通过Agapito-Curtarolo-Buongiorno Nardelli的伪杂化密度泛函自一致地确定的。我们计算了能带结构、铁电畸变、极化、玻恩有效电荷和开关势垒,并与局部密度近似、广义梯度近似(GGA)、元GGA和混合泛函(HSE06)进行了比较。DFT + U + V的结果与实验数据非常吻合,位点间的Hubbard项显著增加了带隙,与GW的结果更加吻合。讨论了位间库仑相互作用恢复被位间U抑制的极性畸变的关键作用。我们的方法产生了与HSE06相当的精度,计算成本降低了一个数量级以上。这种精度和效率的结合使得DFT + U + V非常适合高通量计算和特性,如铁电异质结构的大块光伏效应和带对准。
First principles study of dielectric properties of ferroelectric perovskite oxides with extended Hubbard interactions
We investigate the atomic and electronic structures of ferroelectric perovskite oxides, BaTiO3, PbTiO3, LiNbO3, and BiFeO3 using ab initio extended Hubbard functionals (DFT + U + V), where on-site and inter-site Hubbard parameters are self-consistently determined via a pseudohybrid density functional by Agapito-Curtarolo-Buongiorno Nardelli. We compute band structures, ferroelectric distortions, polarization, Born effective charges, and switching barriers, compared with local density approximation, generalized gradient approximation (GGA), meta-GGA, and hybrid (HSE06) functionals. Results from DFT + U + V closely match experimental data, with the inter-site Hubbard terms significantly increasing band gaps, making closer alignment with GW results. The crucial role of the inter-site Coulomb interactions, restoring polar distortions suppressed by on-site U is discussed. Our approach yields accuracy comparable to HSE06 at over an order-of-magnitude lower computational cost. This combination of accuracy and efficiency makes DFT + U + V well suited for high-throughput calculations and properties such as bulk photovoltaic effect and band alignments of ferroelectric heterostructures.
期刊介绍:
npj Computational Materials is a high-quality open access journal from Nature Research that publishes research papers applying computational approaches for the design of new materials and enhancing our understanding of existing ones. The journal also welcomes papers on new computational techniques and the refinement of current approaches that support these aims, as well as experimental papers that complement computational findings.
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